Process for production of trialkoxyhalosilanes, process for production of alkoxy (dialkylamino) silanes, catalysts for (co)polymerization of a-olefins, catalyst components therefor, and processes for polymerization of a-olefins with the catalysts

ABSTRACT

A process for the production of trialkoxyhalosilanes which comprises reacting a tetrahalosilane [37] with a tetra-alkoxysilane [38] in the presence of an alcohol whose alkoxy group is the same as those of the tetraalkoxysilane to thereby obtain a trialkoxyhalosilane [39], characterized in that the alcohol is used in an amount of 5 to 50% by mole based on the total amount of Si of the tetrahalosilane and the tetraalkoxysilane: SiX 4  [37] (wherein X is halogeno) Si(OR 1 ) 4  [38] (wherein R 1  is a hydrocarbon group having 1 to 6 carbon atoms) XSi(OR 1 ) 3  [39] (wherein X and R 1  are each as defined above).

FIELD OF THE INVENTION

The present invention relates to a novel process for production oftrialkoxyhalosilanes, and a novel process for production ofalkoxy(dialkylamino) silanes. It also relates to a catalyst forpolymerization or copolymerization of α-olefins, a catalyst componenttherefor, and a process for polymerization of α-olefins with thecatalyst.

BACKGROUND OF THE INVENTION

An alkoxy(dialkylamino) silane can be produced in a known process, whichcomprises reacting an alkoxysilane with a Grignard reagent forintroduction of an amino group, and in another known process ofproduction, which uses an alkoxy halosilane as a raw material.

The processes for production of alkoxy halosilanes, which comprisereacting a tetrasilane with an alcohol, are disclosed in Non-PatentDocument 1 (J. Am. Chem. Soc., Vol 68, p. 70, 1946) and Non-PatentDocument 2 (Khimiya i Industriya, No. 6, p. 248, 1983).

Non-Patent Document 1 shows an experimental example using atetrachlorosilane and an allyl alcohol under an experimental conditionto obtain a triallyloxychlorosilane as a major product in which thetetrachlorosilane is reacted with the allyl alcohol at a molar ratio of1:2.5. The yield is 53% and a much higher yield is required, needless tosay. As for other kinds of alkoxychlorosilanes, such as chlorotrimethoxysilane, chlorotriethoxysilane, dichlorodiethoxy silane andtrichloroethoxysilane, though they can be assumably synthesized becauseboiling points and physical property values are described, there is nodescription about yields.

In Non-Patent Document 2, details such as experimental conditions areunavailable. The study abstract described in the chemical abstract No.100:34098 shows that, among chloro ethoxysilanes as alkoxyhalosilanes, atrichloroethoxysilane with introduction of one ethoxy group is obtainedat a yield of 90%, and a dichloroethoxysilane with introduction of twoethoxy groups is obtained at a yield of 95%, but a chloroethoxysilanewith introduction of three ethoxy groups is obtained at a lower yield of80%. Further, the reaction condition described includes reactiontemperatures of 100-145° C., and much lower temperatures are desired.

On the other hand, Patent Document 1 (JP-A 5-310751) proposes a processfor production of alkoxyhalosilanes through reaction of atetrachlorosilane with a tetraalkoxysilane. It shows the use of an acidas a catalyst. An acid with a higher boiling point, however, causesreduction in yield in accordance with separation failures or heatingunder coexistence during distillation, isolation and purification of aproduct. Titanium tetrachloride, aluminum chloride and boron fluorideshown as examples of Lewis acid are sensitive to humidity in theatmosphere and generally have difficulties in handing. On the otherhand, hydrogen halides are gases at room temperature under normalpressure and easily removable from reaction systems. This Document showsdirect introduction into the reaction system and examples of generationin the system by H₂O. In general, however, the need for giving attentionto handing gaseous hydrogen halides increases the cost of the facility.Though the generation in the system by H₂O can be considered safe andless costly, a silane halide is consumed by the extent of introductionof H₂O and converted into a compound having a Si—O bond different fromthe aimed alkoxysilane halide. Accordingly, a problem arises because aSi-based yield is lowered. The more the quantity of the catalyst, themore the reduction in production cost can be desired because of theeffect of shortening the reaction time. In this case, however, the abovemethod requires a large amount of H₂O to be introduced, which inevitablyinvites reduction in yield as a drawback. Examples of Patent Document 1have yields of 60-75% at most and there is a need for processes capableof achieving much higher yields.

With respect to chlorotriethoxysilanes, Non-Patent Document 3 (ZhurnalObshchei Khimii, vol. 65, p. 1142, 1995) discloses that when atetrachlorosilane is reacted with a tetraalkoxysilane under condition ofheating at 40° C. in the presence of 0.02-1.0 wt. % ethanol, ClSi(OEt)₃can be obtained at a maximum yield of 90% based on Cl in the rawmaterial composition. Similar to the yields exemplified in the precedingparagraphs, however, the yield based on Si important on cost computationin the raw material composition is 82%. Accordingly, much higher yieldsare still required. Implementation without humidification is alsodesired.

Non-Patent Document 4 (Trudy Instituta-MoskovskiiKhimiko-Tekhnokogcheskii Institut imeni D. I. Mendeleeva (1972), No. 70140-2) reports that reaction of ClSi(OEt)₃ with Et₂NH yieldsEt₂NSi(OEt)₃. Isolation/purification of ClSi(OEt)₃ is not preferable,however, because it causes substance loss not a little and increasespurification steps.

On the other hand, in recent years, for polymerization of α-olefins,JP-A 57-63310 (Patent Document 2), JP-A 57-63311 (Patent Document 3),JP-A 58-83016 (Patent Document 4), JP-A 59-58010 (Patent Document 5) andJP-A 60-44507 (Patent Document 6) propose many a high-activity carriercatalyst system. The system comprises a solid catalyst componentessentially including magnesium, titanium, a halogen element and anelectron donor; an organometallic compound of a I-III group metal in theperiodic table; and an electron donor. Further, JP-A 62-11705 (PatentDocument 7), JP-A 63-223008 (Patent Document 8), JP-A 63-259807 (PatentDocument 9), JP-A 2-84404 (Patent Document 10), JP-A4-202505 (PatentDocument 11) and JP-A4-370103 (Patent Document 12) disclosepolymerization catalysts characterized by the use of a specificorganosilicon compound as the electron donor. For example, JP-A 2-84404(Patent Document 13) discloses a process in which acyclopentylalkyldimethoxysilane or a dicyclopentyl dimethoxysilane isemployed as the electron donor. The catalyst system using such thesilicon compound is not always excellent in hydrogen response. JP-A63-223008 (Patent Document 14) discloses a catalyst system using a din-propyldimethoxy silane excellent in hydrogen response as the electrondonor. The system can not satisfy stereomainity, however, and has aproblem because the stiffness of an α-olefin polymer can not beenhanced.

JP-A 9-40714 (Patent Document 15) discloses an alkoxysilane compoundhaving an aliphatic amino substituent. JP-A8-3215 (Patent Document 16),JP-A8-100019 (Patent Document 17) and JP-A 8-157519 (Patent Document 18)propose processes for production of α-olefins using an alkoxysilanehaving an aliphatic amino substituent as the catalyst component. Theseprocesses, however, can not always satisfy hydrogen response inperformance particularly. JP-A 8-143620 (Patent Document 19) proposes aprocess for production of α-olefins using a dialkoxysilane having twoaliphatic amino substituents as the electron donor. The process,however, can not always satisfy polymerization activity andstereomainity in performance.

JP-A8-120021 (Patent Document 20), JP-A8-143621 (Patent Document 21) andJP-A 8-231663 (Patent Document 22) disclose processes usingcycloaminosilane compounds. The use of these specifically describedcompounds as the catalyst component can achieve high stereomainity butcan not always satisfy hydrogen response.

The carrier catalyst system using the electron donor can not alwayssatisfy the balance among polymerization activity, stereomainity andhydrogen response in performance. Accordingly, a further improvement isdesired.

In recent years, in the field of injection molding mainly aimed atautomobile materials and household electrical appliance materials, forthe purpose of thinning and light-weighting of goods, there areincreased needs for α-olefin polymers with high melt fluidity, highstiffness and high heat resistance. For production of such the α-olefinpolymers, the use of a catalyst with high hydrogen response is importanton polymerization. Specifically, for adjustment of the molecular weightof an α-olefin polymer, hydrogen is generally employed as a chaintransfer agent that coexists in the polymerization system. Inparticular, elevation of the melt fluidity of the α-olefin polymerrequires the molecular weight lowered by hydrogen. A melt flow rate isemployed as an index for the melt fluidity of the α-olefin polymer. Thelower the molecular weight of the α-olefin polymer, the higher the meltflow rate becomes relationally. Lower hydrogen response requires a largequantity of hydrogen in the polymerization system to elevate the meltflow rate of the α-olefin polymer. To obtain the α-olefin polymer withthe same flow rate, higher hydrogen response does not require thequantity of hydrogen as large as the lower hydrogen response requires.Therefore, the lower hydrogen response requires introduction of anexcessive quantity of hydrogen into the polymerization system to elevatethe melt flow rate of the α-olefin polymer. Accordingly, in productionprocesses, for safety, a polymerization device with a limited resistanceto pressure elevates partial pressure of hydrogen. In such the relation,the polymerization temperature should be lowered, exerting an ill effecton the production speed and the quality as a problem.

The above-described organosilicon compounds are synthesized using anorganometallic reagent such as a Grignard reagent and accordingly theraw material reagent is expensive. Therefore, the use of theorganosilicon compound synthesized in the process to produce an α-olefinpolymer inevitably makes the α-olefin polymer itself expensive andcauses a problem on production cost.

Patent Document 1: JP-A 5-310751

Patent Document 2: JP-A 57-63310

Patent Document 3: JP-A 57-63311

Patent Document 4: JP-A 58-83016

Patent Document 5: JP-A 59-58010

Patent Document 6: JP-A 60-44507

Patent Document 7: JP-A 62-11705

Patent Document 8: JP-A 63-223008

Patent Document 9: JP-A 63-259807

Patent Document 10: JP-A 2-84404

Patent Document 11: JP-A 4-202505

Patent Document 12: JP-A 4-370103

Patent Document 13: JP-A 2-84404

Patent Document 14: JP-A 63-223008

Patent Document 15: JP-A 9-40714

Patent Document 16: JP-A 8-3215

Patent Document 17: JP-A 8-100019

Patent Document 18: JP-A 8-157519

Patent Document 19: JP-A 8-143620

Patent Document 20: JP-A 8-120021

Patent Document 21: JP-A 8-143621

Patent Document 22: JP-A 8-231663

Non-Patent Document 1: J. Am. Chem. Soc., Vol 68, p. 70, 1946

Non-Patent Document 2: Khimiya i Industriya, No. 6, p. 248, 1983

Non-Patent Document 3: (Zhurnal Obshchei Khimii, vol. 65, p. 1142, 1995)

Non-Patent Document 4: Trudy Instituta-MoskovskiiKhimiko-Tekhnokogcheskii Institut imeni D. I. Mendeleeva (1972), No. 70140-2

SUMMARY OF THE INVENTION

Problems to be Solved in the Invention

The present invention solves the problems in the above-describedconventional processes for production of alkoxyhalosilanes and has afirst object to provide a novel process for production oftrialkoxyhalosilanes.

The present invention solves the problems in the above-describedconventional processes for production of alkoxy(dialkylamino)silanes andhas a second object to provide a novel process for production oftrialkoxy(dialkylamino) silanes.

The present invention solves the problems in the above-describedconventional polymerization of α-olefins and has a third object toprovide α-olefin polymers or copolymers with higher hydrogen response,higher polymerization activity, higher stereomainity, better meltfluidity and lower production costs.

Means for Solving The Problems

To achieve the first object, the present invention provides a firstprocess for production of trialkoxyhalosilanes, which comprises reactinga tetrahalosilane represented by Formula 19 with a tetraalkoxysilanerepresented by Formula 20 in the mixture of an alcohol composed of thesame alkoxy group as that of the tetraalkoxysilane to yield atrialkoxyhalosilane represented by Formula 21, wherein the alcohol isused in an amount of 5-50% by mol based on a total amount of Si in thetetrahalosilane and the tetraalkoxysilane.SiX₄  [Formula 19](where X denotes halogen)Si(OR¹)₄  [Formula 20](where R¹ denotes a hydrocarbon group having 1-6 carbon atoms).XSi(OR¹)₃  [Formula 21](where X denotes halogen; and R¹ a hydrocarbon group having 1-6 carbonatoms.)

To achieve the first object, the present invention provides a secondprocess for production of trialkoxyhalosilanes, which comprises reactinga tetrahalosilane represented by Formula 22 with an alcohol representedby Formula 23 at a controlled temperature of 40° C. or below to yield atrialkoxyhalosilane represented by Formula 24.SiX₄  [Formula 22](where X denotes halogen)R¹OH  [Formula 23](where R¹ denotes a hydrocarbon group having 1-6 carbon atoms)XSi(OR¹)₃  [Formula 24](where X denotes halogen; and R¹ a hydrocarbon group having 1-6 carbonatoms).

To achieve the second object, the present invention provides a processfor production of trialkoxy(dialkylamino) silanes, which comprises afirst step including the first or second process for production oftrialkoxyhalosilanes; and a second step of reacting thetrialkoxyhalosilane obtained in the first step with a dialkylaminerepresented by Formula 25 to yield a trialkoxy(dialkylamino)silanerepresented by Formula 26.R²R³ NH  [Formula 25](where R² denotes a hydrocarbon group having 1-12 carbon atoms; and R³ ahydrocarbon group having 1-12 carbon atoms)R²R³NSi(OR¹)₃  [Formula 26](where R¹ denotes a hydrocarbon group having 1-6 carbon atoms; R² ahydrocarbon group having 1-12 carbon atoms; and R³ a hydrocarbon grouphaving 1-12 carbon atoms).

To achieve the third object, the present invention provides a firstcatalyst component for polymerization or copolymerization catalysts ofα-olefins, which comprises a mixture of silane compounds represented byFormulae 27 and 28.Si (OR¹)₃R²  [Formula 27](where R¹ denotes a hydrocarbon group having 1-6 carbon atoms; and R² ahydrocarbon group having 1-12 carbon atoms, an amino group including ahydrogen atom and a hydrocarbon group having 1-12 carbon atoms, whichare bonded on a N atom, or an amino group including two hydrocarbongroups each having 1-12 carbon atoms, which are bonded on a N atom (thetwo hydrocarbon groups may be the same or different from each other))SiR³ ₄  [Formula 28](where R³ denotes an alkoxy group having 1-6 carbon atoms, a hydrocarbongroup having 1-12 carbon atoms, an amino group including a hydrogen atomand a hydrocarbon group having 1-12 carbon atoms, which are bonded on aN atom, or an amino group including two hydrocarbon groups each having1-12 carbon atoms, which are bonded on a N atom (the two hydrocarbongroups may be the same or different from each other). Each R³ may be thesame as or different from another. Formulae 27 and 28 do not representthe same compound).

To achieve the third object, the present invention provides a secondcatalyst component for polymerization or copolymerization catalysts ofα-olefins, which comprises a mixture of silane compounds represented byFormulae 29 and 30.Si(OR¹)₃(NR⁴R⁵)  [Formula 29](where R¹ denotes a hydrocarbon group having 1-6 carbon atoms; R⁴ ahydrocarbon group having 1-12 carbon atoms, or a hydrogen atom; and R⁵ ahydrocarbon group having 1-12 carbon atoms)Si(R⁶)_(n)(NR⁷R⁸)_(4-n)  [Formula 30](where R⁶ denotes a hydrocarbon group having 1-12 carbon atoms or analkoxy group having 1-6 carbon atoms (each R⁶ may be the same as ordifferent from another); R⁷ a hydrocarbon group having 1-12 carbonatoms; R⁸ a hydrocarbon group having 1-12 carbon atoms; and n is equalto 1-2 or 4).

To achieve the third object, the present invention provides a thirdcatalyst component for polymerization or copolymerization catalysts ofα-olefins, which comprises a reacted mixture of a trialkoxyhalosilanerepresented by Formula 35 with a dialkylamine represented by Formula 36.XSi(OR¹)₃  [Formula 35](where X denotes halogen; and R¹ denotes a hydrocarbon group having 1-4carbon atoms)R²R³NH  [Formula 36](where R² denotes a hydrocarbon group having 1-12 carbon atoms; and R³ ahydrocarbon group having 1-12 carbon atoms).Effects of the Invention

The process for production of trialkoxyhalosilanes according to thepresent invention is possible to provide trialkoxyhalosilanes at higheryields.

The process for production of trialkoxy(dialkylamino) silanes accordingto the present invention is possible to providetrialkoxy(dialkylamino)silanes at higher yields.

The catalyst component according to the present invention can beemployed to inexpensively produce α-olefin polymers with higher hydrogenresponse, higher polymerization activity, higher stereomainity andbetter melt fluidity. Particularly, the greatly improved hydrogenresponse over the conventional catalyst systems allows α-olefin polymerswith high stiffness and nice melt fluidity to be produced at nosacrifice of productivity. The use of the catalyst system of the presentinvention allows production of an ethylene-propylene copolymer at ablock rate of 10-50 wt. % and production of a reactor-made TPO. Theorganosilicon compound of the catalyst component of the presentinvention does not contain the conventional expensive organometalliccompound and the distillation/purification process on synthesis of thecatalyst component can be simplified. Therefore, it is possible tosynthesize an organosilicon compound at a lower production cost. In aword, the use of the catalyst component of the present invention allowsproduction of α-olefin polymers inexpensively.

BRIEF DESCRIPTION OF THE DRAWINGS

[FIG. 1] is a flowchart showing a preparation process and polymerizationmethod of a catalyst component of the present invention.

[FIG. 2] shows a mass spectrum of a diethylamine.

[FIG. 3] shows a mass spectrum of a tetraethoxysilane.

[FIG. 4] shows a mass spectrum of a diethylaminodiethoxy methoxysilane.

[FIG. 5] shows amass spectrum of a diethylaminotriethoxy silane.

[FIG. 6] shows a mass spectrum of a bis(diethylamino)diethoxy silane.

[FIG. 7] shows a mass spectrum of a hexaethoxydisiloxane.

DETAILED DESCRIPTION OF THE INVENTION

First Process for Production of Trialkoxyhalosilanes

A first process for production of trialkoxyhalosilanes employs thetetrahalosilane represented by Formula 19, such as tetrafluorosilane,tetrachlorosilane and tetrabromosilane. The tetrachlorosilane ispreferable among those.

In the tetraalkoxyhalosilane represented by Formula 20, R1 is ahydrocarbon group having 1-6, preferably 2-6, more preferably 2-4 carbonatoms. The tetraalkoxyhalosilane represented by Formula 20 includestetramethoxysilane, tetraethoxysilane, tetra-n-propoxysilane,tetra-iso-propoxy silane, tetra-n-butoxysilane andtetra-tert-butoxysilane. The tetraethoxysilane is preferable amongthose.

Though the first process for production of trialkoxyhalosilanes canproceed with no solvent, it may be performed with the use of a solventthat can not react with the raw material and the reacted product. When asolvent is employed, the solvent may include n-hexane, n-heptane,toluene, and diethyl ether.

The alcohol for use in the reaction system in the first process forproduction of trialkoxyhalosilanes reacts with a tetrahalosilane in thereaction system including the tetrahalo silane represented by Formula 19and the tetraalkoxysilane represented by Formula 20 to generate ahydrogen halide in accordance with Expression 1.nROH+SiX₄→X_((4-n))Si(OR)_(n)+nHX(n=1-4)  [Expression 1]

In the reaction system including the tetrahalosilane represented byFormula 19, the tetraalkoxysilane represented by Formula 20 and analcohol, an initial mixture can be expressed, based on a reactionequation obtained by substitution of n=4 into Expression 1, formally asa mixture of: a tetrahalosilane decreased by the extent equal to 0.25times the molar quantity of the used alcohol; a tetraalkoxysilaneincreased by the extent equal to 0.25 times the molar quantity; and ahydrogen halide equal to an equivalent molar quantity of the alcohol.This reacted mixture can be converted into an equilibrated mixture ofX_((4-m))Si(OR)_(m) (where m=0-4). The generated hydrogen halide has anexcellent catalytic action on interconversion of X_((4-m))Si(OR)_(m)(where m=0-4). The use of the action achieves an effect on shorteningthe reaction time. Therefore, it is extremely desirable to keep thehydrogen halide in the reaction system. In a word, the first process forproduction of trialkoxyhalosilanes according to the present invention ispreferably performed in the presence of an acid catalyst. Preferably,the acid catalyst is the hydrogen halide secondarily produced in thereaction.

A molar ratio of the tetrahalosilane represented by Formula 19 to thetetraalkoxysilane represented by Formula 20 is preferably 1:2.6 to 1:3.8after the formal chemical conversion shown in the preceding paragraph.It is more preferably 1:3.0 to 1:3.4, and particularly preferably morethan 1:3, in which a molar quantity of the tetraalkoxysilane in use ismore than three times the molar quantity of the tetrahalosilane in use.

The amount of the alcohol for use in reaction is preferably 5-50% bymol, more preferably 10-30% by mol based on a total amount of Si in thetetrahalosilane represented by Formula 19 and the tetraalkoxysilanerepresented by Formula 20. A smaller amount in use than this range slowsthe reaction and a larger amount in use than this range lowers theyield.

In the first process of production of trialkoxyhalo silanes, a reactiontemperature is preferably between −20 and 80° C., more preferablybetween 0 and 50° C. A lower temperature than this range slows thereaction and a higher temperature than this range lowers the solubilityof the generated hydrogen halide undesirably. Preferably, the reactiontime is 0.05-6.0 hrs.

Second Process for Production of Trialkoxyhalosilanes

A second process for production of trialkoxyhalosilanes employs thetetrahalosilane represented by Formula 22, such as tetrafluorosilane,tetrachlorosilane and tetrabromosilane. The tetrachlorosilane ispreferable among those.

In the alcohol represented by Formula 23, R¹ is a hydrocarbon grouphaving 1-6, preferably 2-6, and more preferably 2-4 carbon atoms. Thealcohol represented by Formula 23 includes methanol, ethanol,1-propanol, 2-propanol, and 1-butanol. The ethanol is preferable amongthose.

Though the reaction of the tetrahalosilane represented by Formula 22with the alcohol represented by Formula 23 can proceed with no solventit may proceed with the use of a solvent that can not react with the rawmaterial and the reacted product. If a solvent is employed, the solventmay include n-hexane, n-heptane, toluene, and diethylether.

The reaction of the tetrahalosilane represented by Formula 22 with thealcohol represented by Formula 23 is an exothermic reaction thatgenerates the hydrogen halide in accordance with the above Expression 1.This reaction converts the raw material of the tetrahalosilanerepresented by Formula 22 into an equilibrated mixture ofX_((4-m))Si(OR)_(m) (where m=0-4). The generated hydrogen halide has anexcellent catalytic action on interconversion of X_((4-m))Si(OR)_(m)(where m=0-4). The use of the action achieves an effect on shorteningthe reaction time. Therefore, it is extremely desirable to keep thehydrogen halide in the reaction system. In a word, the second processfor production of trialkoxyhalosilanes according to the presentinvention is preferably performed in the presence of an acid catalyst.Preferably, the acid catalyst is the hydrogen halide secondarilyproduced in the reaction.

On the other hand, the solution of the hydrogen halide into the reactedproduct is an endothermic reaction. Through various studies on mixingmethods and reaction containers, an unconventional condition has beenfound on controlling heat absorbing/radiating in accordance with thereaction using no special cooling machine to proceed the reaction at alow temperature in a short time. Namely, the hydrogen halide of thepresent invention has a reaction accelerating effect and a self-coolingeffect.

A reaction temperature is preferably −50 to 40° C., and most preferably−20 to 30° C. from the viewpoint of no need for a special coolingfacility. In a word, in the second process for production oftrialkoxyhalosilanes, the reaction temperature is preferablycontrollable with no special cooling facility. Cooling down to −20° C.can be achieved by self-cooling or without cooling from external if heatabsorbing in accordance with the solution of the hydrogen halide isutilized effectively. This is very preferable with respect to cost. Theeffective utilization of heat absorbing in accordance with the solutionnaturally increases the solved quantity of the hydrogen halide andexerts the reaction time shortening effect due to the catalytic action.On the other hand, at 40° C. or higher, dehydrohalogenation from thereacted solution becomes remarkable to eliminate the reaction timeshortening effect. Though suppression of dehydrohalogenation can besolved if the reaction container has a pressure-proof hermeticstructure, it requires a corresponding extra cost and results in asafety cost undesirably.

A reaction time is usually 0.25-72 hrs and controllable depending on thetypes and amounts of the tetrahalosilane and the alcohol as well as thereaction temperatures, preferably 0.25-3 hrs. Depending on the cases, itis preferable to execute a reaction at −20 to 5° C. for 0.25-24 hrs andthen a reaction at 10 to 30° C. for 0.25-72 hrs.

A molar ratio of the tetrahalosilane represented by Formula 22 to thealcohol represented by Formula 23 is preferably 1:2.6 to 1:3.3, and morepreferably 1:2.8 to 1:3.1.

Process for Production of Trialkoxy(Dialkylamino) Silanes

In the process for production of trialkoxy(dialkylamino) silanesaccording to the present invention, the reacted mixture obtained in thefirst step is preferably reacted with the dialkylamine represented byFormula 25 without isolation and purification.

In the process for production of trialkoxy(dialkylamino) silanesaccording to the present invention, the dialkylamine represented byFormula 25 may include dimethylamine, diethyl amine, dibutylamine andmethylethylamine. The diethylamine is preferable among those.

In the dialkylamine represented by Formula 25, R² and R³ denote ahydrocarbon group having 1-12, preferably 1-4 carbon atoms. In thesecond step of the process for production oftrialkoxy(dialkylamino)silanes according to the present invention, ifthe dialkylamine represented by Formula 25 is inexpensive, a method withthe use of a greatly excessive amount of the dialkylamine represented byFormula 25 is simple and preferable, also serving capture of thehydrogen halide produced in the reaction. When an excessive amount ofthe dialkylamine represented by Formula 25 is not employed, for thepurpose of capture of the hydrogen halide produced in the reaction, atertiary amine, such as triethylamine and N-ethyl-diisopropylamine, or apyridine may be mixed. A reaction temperature is preferably −20 to 200°C., more preferably 0 to 120° C., and most preferably 10 to 80° C. fromthe viewpoint of no need for a heating or cooling facility. If thereaction temperature exceeds the boiling point, an inert gas such asnitrogen and argon may be employed to pressurize. A reaction time may be0.25-120 hrs, preferably 0.25-3 hrs.

First or Second Catalyst Component for Polymerization orCopolymerization Catalysts of α-olefins

In the first catalyst component for polymerization or copolymerizationcatalysts of α-olefins according to the present invention, R¹ in Formula27 denotes a hydrocarbon group having 1-6, preferably 2-6 carbon atoms,which may include an unsaturated or saturated aliphatic hydrocarbongroup having 1-6 carbon atoms. Specific examples may include methylgroup, ethyl group, n-propyl group, isopropyl group, n-butyl group,isobutyl group, t-butyl group, and s-butyl group. The ethyl group isparticularly preferable.

In Formula 27, R² is a hydrocarbon group having 1-12 carbon atoms, anamino group including a hydrogen atom and a hydrocarbon group having1-12 carbon atoms, which are bonded on a N atom, or an amino groupincluding two hydrocarbon groups each having 1-12 carbon atoms, whichare bonded on a N atom (the two hydrocarbon groups may be the same ordifferent from each other). Specific examples may include methyl group,ethyl group, propyl group, methylamino group, dimethylamino group,methylethylamino group, diethylamino group, ethyl n-propyl amino group,ethylisopropylamino group, methyl n-propylamino group,methylisopropylamino group, 1,2,3,4-tetrahydroquinolyl group,1,2,3,4-tetrahydroisoquinolyl group, perhydro quinolyl group, andperhydroisoquinolyl group. The diethyl amino group is particularlypreferable.

In the first or second catalyst component for polymerization orcopolymerization catalysts of α-olefins according to the presentinvention, the organosilicon compound component represented by Formula27 or 33 may include dimethylaminotriethoxysilane,diethylaminotriethoxysilane, diethylaminotrimethoxysilane,diethylaminotri n-propoxy silane, di n-propylaminotriethoxysilane,methyl n-propylamino triethoxysilane, t-butylaminotriethoxysilane, ethyln-propylaminotriethoxysilane, ethylisopropylaminotriethoxy silane, andmethylethylaminotriethoxysilane. Preferably, it may includediethylaminotriethoxysilane and diethylamino trimethoxysilane. Theseoroganosilicon compounds may be employed solely or in combination of twoor more.

The organosilicon compound component represented by Formula 28 or 34 mayinclude bisaminosilanes such as bis(dimethylamino)diethoxysilane,bis(diethylamino)diethoxy silane, bis(diethylamino)dimethoxysilane,bis(diethylamino) di n-propoxysilane, bis(din-propylamino)diethoxysilane, bis(methyl n-propylamino)diethoxysilane,bis(t-butylamino) diethoxysilane, bis(ethyln-propylamino)diethoxysilane, bis (ethylisopropylamino)diethoxysilane,and bis(methylethyl amino)diethoxysilane. It may also includetetraalkoxysilanes such as tetramethoxysilane, tetraethoxysilane, tetran-propoxysilane, tetraisopropoxysilane, tetra n-butoxysilane,tetraisobutoxysilane, tetra s-butoxysilane, and tetra t-butoxysilane. Itmay further include ethyltrimethoxysilane, methyldiethoxysilane,ethyldimethoxysilane, methyltriethoxy silane, dimethoxydiethoxysilane,ethyldiethoxysilane, tri ethoxymethoxysilane, ethyltriethoxysilane, anddiethylamino diethoxysilane. These organosilicon compounds may beemployed solely or in combination of two or more.

In the first or second catalyst component for polymerization orcopolymerization catalysts of α-olefins according to the presentinvention, the silane compound represented by Formulae 27-34 may besynthesized by reacting a tetrahalosilane represented by Formula 31 witha tetraalkoxysilane represented by Formula 32 to yield atrialkoxyhalosilane represented by Formula 33, which is then reactedwith a dialkylamine represented by Formula 34. In this synthesis, thereaction of the tetrahalosilane represented by Formula 31 with thetetraalkoxysilane represented by Formula 32 is performed preferably inthe presence of an acid catalyst.SiX₄  [Formula 31](where X denotes halogen)Si(OR¹)₄  [Formula 32](where R¹ denotes a hydrocarbon group having 1-6, preferably 2-6 carbonatoms)XSi(OR¹)₃  [Formula 33](where X denotes halogen; and R¹ a hydrocarbon group having 1-6,preferably 2-6 carbon atoms)R²R³NH  [Formula 34](where R² denotes a hydrocarbon group having 1-12 carbon atoms; and R³ ahydrocarbon group having 1-12 carbon atoms).

A diethylaminotriethoxysilane, or the first or second catalyst componentfor polymerization or copolymerization catalysts of α-olefins accordingto the present invention, may be synthesized in the presence of an acidcatalyst by reacting a tetrachlorosilane with a tetraethoxysilane at amolar ratio of 1:3 to yield a chlorotriethoxysilane, subsequentlyreacting a diethylamine with the chlorotriethoxysilane equivalently. Atthe same time, bis(diethylamino)diethoxysilane, tris(diethylamino)ethoxysilane, and hexaethoxydisiloxane may be producedsecondarily.

Third Catalyst Component for Polymerization or CopolymerizationCatalysts of α-Olefins

In the third catalyst component for polymerization or copolymerizationcatalysts of α-olefins according to the present invention, the reactedmixture component of the trialkoxyhalosilane represented by Formula 35with the dialkylamine represented by Formula 36 can be employed withoutisolation and purification. For example, the reacted mixture ofXSi(OR¹)₃ with R²R³NH may be employed in polymerization while it is notfiltered and accordingly still contains a secondary product ofR²R³NH—HCl. The XSi(OR¹)₃ and R²R³NH may employ a reacted product addedand mixed in the polymerization bath as a (C) component.

In the trialkoxyhalosilane represented by Formula 35, R¹ is ahydrocarbon group having 1-6, preferably 2-6 carbon atoms, which mayinclude an unsaturated or saturated aliphatic hydrocarbon group having1-6 carbon atoms. Specific examples may include methyl group, ethylgroup, n-propyl group, isopropyl group, n-butyl group, isobutyl group,t-butyl group, and s-butyl group. The ethyl group is particularlypreferable.

In the trialkoxyhalosilane represented by Formula 35, X is halogen,preferably chlor. The trialkoxyhalosilane represented by Formula 35includes specific examples such as chlortriethoxysilane,chlortrimethoxysilane, and chlortri n-propoxysilane.

In the dialkylamine represented by Formula 36, R² or R³ is a hydrocarbongroup having 1-12 carbon atoms, which may include an unsaturated orsaturated aliphatic hydrocarbon group having 1-12 carbon atoms. Specificexamples may include methyl group, ethyl group, n-propyl group,isopropyl group, n-butyl group, isobutyl group, t-butyl group, ands-butyl group. The ethyl group is particularly preferable. Thedialkylamine represented by Formula 36 may include a diethylamine as aspecific example.

Polymerization or Copolymerization Catalysts of α-Olefins

The present invention also provides a polymerization or copolymerizationcatalyst of α-olefins, which contains the first through third catalystcomponent for polymerization or copolymerization catalysts of α-olefins.The present invention further provides a polymerization orcopolymerization catalyst of α-olefins, which comprises [A] a solidcatalyst component essentially including magnesium, titanium, a halogenelement and an electron donor; [B] an organoaluminum compound component;and [C] the first through third catalyst component for polymerization orcopolymerization catalysts of α-olefins.

The present invention employs a solid catalyst component essentiallyincluding magnesium, titanium, a halogen element and an electron donoras the component [A]. The process for production of the solid catalystcomponent of the component [A] is not limited particularly. For example,available processes are proposed in JP-A54-94590, JP-A5-55405,JP-A56-45909, JP-A 56-163102, JP-A 57-63310, JP-A 57-115408, JP-A58-83006, JP-A 58-83016, JP-A 58-138707, JP-A 59-149905, JP-A 60-23404,JP-A 60-32805, JP-A 61-18330, JP-A 61-55104, JP-A 63-3010, JP-A1-315406, JP-A 2-77413 and JP-A 2-117905.

Typical processes for production of the solid catalyst component [A] arelisted as follows. (1) A process comprises pulverizing a magnesiumcompound, an electron donor and a titanium halide compound together, ordispersing and solving them in solvent, to bring them in contact witheach other for preparation. (2) A process comprises solving a magnesiumcompound and an electron donor in solvent such as toluene, and adding atitanium halide compound into the solution for reaction to precipitate acatalyst solid.

The magnesium compound available for preparation of the solid catalystcomponent [A] includes magnesium halide and dialkoxy magnesium. Themagnesium halide specifically includes magnesium chloride, magnesiumbromide, magnesium iodide, and magnesium fluoride. Particularly, themagnesium chloride is preferable. The dialkoxy magnesium specificallyincludes dimethoxy magnesium, diethoxy magnesium, di n-propoxymagnesium, di n-butoxy magnesium, ethoxymethoxy magnesium, ethoxyn-propoxy magnesium, and buthoxyethoxy magnesium. Particularly, thediethoxy magnesium and the di n-butoxy magnesium are preferable. Thedialkoxy magnesium may also be prepared by reacting metal magnesium withalcohol in the presence of halogen or a halogen-containing metalcompound. The above dialkoxy magnesium may be employed solely or incombination of two or more.

The dialkoxy magnesium available for preparation of the solid catalystcomponent [A] may be shaped granular, powdery, indeterminate orspherical. For example, the use of the spherical dialkoxy magnesiumleads to production of powders of α-olefin homopolymers or copolymerswith other α-olefins, which are excellent in morphology and have anarrow particle diameter distribution. The powders are excellent inpowder fluidity and accordingly can lead to solution of the problemabout clogging hoppers and lines on production.

The titanium halide compound available for preparation of the solidcatalyst component [A] includes specific examples of: tetrahalidetitanium such as tetrachloro titanium, and tetrabromo titanium;trihalidealkoxy titanium such as trichloromethoxy titanium,trichloroethoxy titanium, trichloropropoxy titanium, trichlorobutoxytitanium, tribromomethoxy titanium, tribromoethoxy titanium,tribromopropoxy titanium, and tribromobuthoxy titanium; dihalidealkoxytitanium such as dichlorodimethoxy titanium, dichlorodiethoxy titanium,dichlorodipropoxy titanium, and dichlorodibutoxy titanium; andhalidetrialkoxy titanium such as chlorotrimethoxy titanium,chlorotriethoxy titanium, chlorotripropoxy titanium, and chlorotributoxytitanium. In particular, the tetrachloro titanium is preferable. Thesetitanium halide compounds may be employed solely or in combination oftwo or more.

The electron donor available for preparation of the solid catalystcomponent [A] includes a Lewis basic compound, preferably an aromaticdiester, preferably a diester orthophthalate. The diester orthophthalateincludes specific examples of dimethyl orthophthalate, methylethylorthophthalate, diethyl orthophthalate, ethyl n-propyl orthophthalate,di n-propyl orthophthalate, n-butyl n-propyl orthophthalate,n-butylethyl orthophthalate, isobutylethyl orthophthalate, di n-butylorthophthalate, diisobutyl orthophthalate, n-pentyl orthophthalate,diisopentyl orthophthalate, di n-hexyl orthophthalate, bis 2-ethylhexylorthophthalate, di n-heptyl orthophthalate, and di n-octylorthophthalate. In particular, the diethylorthophthalate, the din-propyl orthophthalate, the di n-butyl orthophthalate, the diisobutylorthophthalate, the di n-heptyl orthophthalate, the bis 2-ethylhexylorthophthalate, and the di n-octyl orthophthalate are preferable. Thesediester orthophthalates may be employed solely or in combination of twoor more.

JP-A 3-706, JP-A 3-62805, JP-A 4-270705 and JP-A 6-25332 disclosecompounds having two or more ether groups, which may be preferablyemployed as the electron donor. In addition, WO 00/39171 discloses adiester maleate having a straight or branched chain alkyl group with 2-8carbon atoms. Among these diester maleates, di n-butyl maleate isparticularly preferable.

The organoaluminum compound component [B] of the present invention mayinclude alkyl aluminum or alkyl aluminum halide such as diethyl aluminumchloride, preferably alkyl aluminum, specifically trialkyl aluminum,which include specific examples of trimethyl aluminum, triethylaluminum, tri n-propyl aluminum, tri n-butyl aluminum, triisobutylaluminum, tri n-hexyl aluminum, and tri n-octyl aluminum. Among those,the triethyl aluminum is particularly preferable. These organoaluminumcompound components may be employed solely or in mixture of two or more.Similarly, polyaluminoxan obtained through reaction of alkyl aluminumwith water may be employed.

A usage of the organoaluminum compound component [B] as a polymerizationcatalyst of α-olefins is 0.1-2000, preferably 50-1000 by molar ratio ofthe solid catalyst component [A] to titanium (Al/Ti).

In the present invention, a mixture of the organosilicon compoundrepresented by the Expression (1) with the organosilicon compoundrepresented by the Expression (2) as the component [C] is added to theabove [A] and [B] to form a catalyst system, in which α-olefins can bepolymerized or copolymerized.

A usage of the component [C] is 0.001-10, preferably 0.005-5, andparticularly preferably 0.01-1 by molar ratio of the component [B] toaluminum (Si/Al).

The process for polymerization of α-olefins in the present invention mayinclude the following. A slurry polymerization process employs anonpolar solvent such as propane, n-butane, n-pentane, n-hexane,n-heptane and n-octane. A vapor phase polymerization process bringsgaseous monomers into contact with a catalyst for polymerization. A bulkpolymerization process employs liquid monomers as a solvent forpolymerization therein. In the above polymerization processes, eithercontinuous polymerization or batch polymerization may be applied, andpolymerization reaction may be implemented at a single stage or atmultiple stages in combination of the above polymerization processes.

Polymerization of α-Olefins

The present invention provides a process for polymerization ofα-olefins, which comprises polymerizing or copolymerizing an α-olefin inthe presence of the above catalyst.

In the above polymerization process, polymerization pressure is 0.1-20MPa, preferably 0.5-6 MPa. A polymerization temperature is 10-150° C.,preferably 30-100° C., and particularly preferably 60-90° C. Apolymerization time is usually 0.1-10 hours, preferably 0.5-7 hours.When the third catalyst component for polymerization or copolymerizationcatalysts of α-olefins is employed as the catalyst component [C], it ispreferable to react and mix the trialkoxyhalosilane represented byFormula 35 with the dialkylamine represented by Formula 36 and thenbring the reacted mixture into contact with the organoaluminum compoundcomponent [B].

In the present invention, it is preferable to execute preliminarypolymerization of ethyleneorα-olefin in accordance with the abovevarious polymerization processes, followed by main polymerization ofα-olefin. The preliminary polymerization has effects on improvement inpolymerization activity, improvement in stereomainity in polymers, andstabilization of morphology in polymers. The solid catalyst component[A] can be brought into contact with the organoaluminum compoundcomponent [B] and the component [C] previously to polymerize a limitedamount of ethylene or α-olefin for preparation of a preliminarilypolymerized solid. Depending on the cases, instead of polymerizingethylene or α-olefin, a preliminarily processed solid can be prepared bybringing the solid catalyst component [A] into contact with theorganoaluminum compound component [B] and the component [C].

In a contact process of the present invention, the component [A], thecomponent [B] and the component [C] are mixed for reaction usually at0-100° C. for 0.1-100 hours. Though each component may be mixed in ordernot particularly limited, an order of the component [A], the component[B] and the component [C] is preferable. After the contact process, thesolid is cleaned, filtered and separated using an inert hydrocarbonsolvent such as n-heptane and employed as the catalyst solid componentin the preliminary or main polymerization.

The preliminary polymerization of the present invention can be achievedthrough a vapor phase polymerization process, a slurry polymerizationprocess or a bulk polymerization process. The solid resulted from thepreliminary polymerization may be separated and then employed in mainpolymerization or continuously subjected to main polymerization withoutseparation.

A preliminary polymerization time is usually 0.1-10 hours and thepreliminary polymerization is preferably continued until preliminarypolymers are produced in an amount of 0.1-100 g per 1 g of the catalystsolid component. An amount less than 0.1 g per 1 g of the catalyst solidcomponent results in insufficient main polymerization activity, largercatalyst residue, and insufficient stereomainity of α-olefin polymers.An amount more than 100 g may result in lowered polymerization activityand lowered crystallinity of α-olefin polymers. A preliminarypolymerization temperature is 0-100° C., preferably 10-70° C. and thepreliminary polymerization is performed in the presence of each catalystcomponent. When preliminary polymerization is performed at a temperaturehigher than 50° C., it is preferable to reduce the ethylene or α-olefinconcentration or shorten the polymerization time. Otherwise, it isdifficult to control generation of preliminary polymers in an amount of0.1-100 g per 1 g of the catalyst solid component. In addition, thepolymerization activity may lower in the main polymerization and thecrystallinity of resultant α-olefin polymers may lower.

A usage of the organoaluminum compound component [B] on preliminarypolymerization is usually 0.5-1000, preferably 1-100 by Al/Ti molarratio of the solid catalyst component [A] to titanium. A usage ofdiethylamino triethoxysilane of the component [C] is usually 0.01-5,preferably 0.05-1 by Si/Ti molar ratio to aluminum of the component [B].On preliminary polymerization, hydrogen may be allowed to coexist, ifrequired.

In the present invention, a chain transfer agent such as hydrogen may beemployed. A usage of hydrogen required to produce α-olefin polymershaving desired stereomainity, melting point and molecular weight can bedetermined appropriately based on the polymerization process andcondition but usually within a range of hydrogen partial pressurebetween 0.05-3.

In the present invention, α-olefins may include ethylene, propylene,1-butene, 1-hexene, and 4-methylpentene-1,3-methylbutene-1,1-octene. Inthe present invention, for the purposes of lowering the heat sealtemperatures of films, lowering the melting points, and improving thetransparency of films, they may be copolymerized with other α-olefins.

In addition, to enhance the low-temperature impact strength of moldingsoriginated from α-olefin polymers, a block copolymer may be producedthrough copolymerization with another two or more α-olefins afterhomopolymerization of the α-olefins or copolymerization with otherα-olefins.

Production of an ethylene-propylene copolymer specifically includes afirst step of homopolymerization of propylene or copolymerization ofethylene with propylene, and a subsequent second step ofcopolymerization of ethylene with propylene. Further, multistagepolymerization may be performed in both the first and second steps. Thepolypropylene resulted from the first step has a melt flow rate rangingbetween 0.1-2000, preferably 30-1000, and particularly preferably100-700. The polypropylene resulted from the first step hasstereomainity, which is 97.5% or more, preferably 98.0% or more, andparticularly preferably 98.2% or more by meso pentad fraction (mmmm).The copolymer of ethylene with propylene produced in the second step hasa proportion (block rate=(Yield of the copolymer of ethylene withpropylene/Total amount of polymers)×100)) ranging between 1-50 wt. %,preferably 5-35 wt. %.

The catalyst system in the present invention has better hydrogenresponse, higher polymerization activity, higher stereomainity ofresultant α-olefin polymers and better melt fluidity.

The α-olefin polymer resulted from the present invention has higherstereomainity and accordingly is excellent in mechanical physicalproperties such as stiffness, heat-resistance and tensile strength ofinjection moldings, which are beneficial in thinning of injectionmoldings. In addition, it has better melt fluidity and accordingly ispossible to shorten the injection molding cycles and resolve appearancefailures of moldings such as typical flow marks of injection moldings.Further, the block copolymers with other α-olefins can impart impactresistance. Thus, it is possible to obtain α-olefin polymers excellentin melt fluidity and in balance between stiffness and impact resistance.The α-olefin polymers resulted from the present invention is employednot only solely. It may also employed as a compound material in blendwith other plastics and elastomers, and further in mixture with areinforcement of inorganic or organic filler such as glass fibers andtalc or with a crystal nucleus agent. Thus, it is possible to exertexcellent performances as structural materials for automobile andhousehold electric appliance though it is not limited.

EXAMPLE 1

Commercially available 0.145 mol of Si(OEt)₄ and 0.020 mol of EtOH aresupplied into a 100 ml flask with previously nitrogen-replaced internalambient and agitated at room temperature, followed by dropping 0.050 molof SiCl₄ therein. When EtOH is employed in reaction, it reacts withSiCl₄ to generate Si(OEt)₄ and HCl in the system formally in accordancewith 4EtOH+SiCl₄→Si(OEt)₄+4HCl. Based on the substance conversion bythis expression, a substantial raw material composition is calculated tofind that SiCl₄:Si(OEt)₄=1:3.33 and that the quantity of the catalyst is10 mol %. After leaving through the night, the reacted mixture isanalyzed in gas chromatography to find generation of ClSi(OEt)₃ in anamount of 86% based on prepared Si. Additionally, 80 ml of diethylamineand 500 ml of dehydrated heptane are supplied into a 1000 ml flask withpreviously nitrogen-replaced internal ambient and, into the solution,the resultant reacted mixture is dropped and agitated for two hours atroom temperature. Thereafter, the reacted mixture is analyzed in gaschromatography to find generation of Et₂NSi(OEt)₃ in an amount of 75%based on prepared Si.

REFERENTIAL EXAMPLE 1

Commercially available 0.050 mol of ClSi(OEt)₃ (96% gas chromatographypurity) is reacted with 0.050 mol of diethylamine in the presence of0.10 mol of triethylamine in 100 ml of heptane at room temperaturethrough the night. As a result, gas chromatography confirms generationof a mixture containing the targeted triethoxy(diethylamino)silane 93%and a tetraethoxysilane 6%.

From the results of Example 1 and Referential Example 1, it can bedetermined that the amination reaction at the second step in thecontinuous reactions proceeds by about 93±3% in consideration ofaccuracy of the gas chromatography analysis. It is obvious that theyield at the first step in the continuous reactions is substantially alarge factor that varies the yield as a whole. Therefore, in thefollowing Examples 2-8, the first step in the continuous reactions, thatis, production of trialkoxyhalosilanes, is described.

EXAMPLE 2

Commercially available 0.150 mol of Si(OEt)₄ and 0.020 mol of EtOH aresupplied into a 100 ml flask with previously nitrogen-replaced internalambient and agitated at room temperature, dropping 0.050 mol of SiCl₄therein. A substantial raw material composition is SiCl₄:Si(OEt)₄=1:3.44 and the quantity of the catalyst is 10 mol. Afterleaving through the night, the reacted mixture is analyzed in gaschromatography to find generation of 82% ClSi(OEt)₃ and residue of 11%Si(OEt)₄ based on prepared Si.

EXAMPLE 3

The reaction is similarly performed as in Example 2 except that 0.170mol of Si(OEt)₄ is employed instead of 0.150 mol of Si(OEt)₄. Asubstantial raw material composition is SiCl₄: Si(OEt)₄=1:3.89 and thequantity of the catalyst is 9 mol %. The product is analyzed to findgeneration of 77% ClSi(OEt)₃ and residue of 19% Si(OEt)₄ based onprepared Si.

EXAMPLE 4

The reaction is similarly performed as in Example 2 except that 0.155mol of Si(OEt)₄ is employed instead of 0.150 mol of Si(OEt)₄. Asubstantial raw material composition is SiCl₄: Si(OEt)₄=1:3.56 and thequantity of the catalyst is 10 mol %. The product is analyzed to findgeneration of 79% ClSi(OEt)₃ and residue of 12% Si(OEt)₄ based onprepared Si.

EXAMPLE 5

The reaction is similarly performed as in Example 2 except that 0.140mol of Si(OEt)₄ is employed instead of 0.150 mol of Si(OEt)₄. Asubstantial raw material composition is SiCl₄: Si(OEt)₄=1:3.22 and thequantity of the catalyst is 11 mol %. The product is analyzed to findgeneration of 81% ClSi(OEt)₃ and residue of 13% Si(OEt)₄ based onprepared Si.

EXAMPLE 6

The reaction is similarly performed as in Example 2 except that 0.135mol of Si(OEt)₄ is employed instead of 0.150 mol of Si(OEt)₄. Asubstantial raw material composition is SiCl₄: Si(OEt)₄=1:3.11 and thequantity of the catalyst is 11 mol %. The product is analyzed to findgeneration of 85% ClSi(OEt)₃ and residue of 10% Si(OEt)₄ based onprepared Si.

EXAMPLE 7

The reaction is similarly performed as in Example 2 except that 0.130mol of Si(OEt)₄ is employed instead of 0.150 mol of Si(OEt)₄. Asubstantial raw material composition is SiCl₄: Si(OEt)₄=1:3.00 and thequantity of the catalyst is 11 mol %. The product is analyzed to findgeneration of 84% ClSi(OEt)₃ and residue of 11% Si(OEt)₄ based onprepared Si.

EXAMPLE 8

The reaction is similarly performed as in Example 2 except that 0.115mol of Si(OEt)₄ is employed instead of 0.150 mol of Si(OEt)₄. Asubstantial raw material composition is SiCl₄: Si(OEt)₄=1:2.67 and thequantity of the catalyst is 12 mol %. The product is analyzed to findgeneration of 75% ClSi(OEt)₃ and residue of 7% Si(OEt)₄ based onprepared Si.

COMPARATIVE EXAMPLE 1

Commercially available 0.167 mol of Si(OEt)₄ and 0.020 mol of trifluoroacetate are supplied into a 100 ml flask with previouslynitrogen-replaced internal ambient and agitated at room temperature,dropping 0.050 mol of SiCl₄ therein. A raw material composition isSiCl₄: Si(OEt)₄=1:3.33 and the quantity of the catalyst is 9 mol %.After leaving through the night, the reacted mixture is analyzed in gaschromatography to find generation of 73% ClSi(OEt)₃ and residue of 16%Si(OEt)₄ based on prepared Si.

COMPARATIVE EXAMPLE 2

The reaction is similarly performed as in Comparative Example 1 exceptthat 0.020 mol of acetic acid is employed instead of 0.020 mol oftrifluoro acetate. After leaving through the night, the reacted mixtureis analyzed in gas chromatography to find generation of 61% ClSi(OEt)₃and residue of 20% Si(OEt)₄ based on prepared Si.

COMPARATIVE EXAMPLE 3

The reaction is similarly performed as in Comparative Example 1 exceptthat sulfuric acid carrier silica (0.010 mol as an amount of sulfuricacid) is employed instead of 0.020 mol of trifluoro acetate. Afterleaving through the night, the reacted mixture is analyzed in gaschromatography to find generation of 27% ClSi(OEt)₃ and residue of 18%Si(OEt)₄ based on prepared Si.

EXAMPLE 9

In a 500 ml four-neck flask equipped with a nitrogen introduction tube,a thermometer and a dropping funnel, 139.9 g (0.669 mol) oftetraethoxysilane and 9.2 g (21 mol % based on a total amount of Si)(0.20 mol) are prepared and water-cooled, dropping 46.5 g (0.274 mol) oftetrachlorosilane therein for 10 minutes in nitrogen ambient. Aftercompletion of dropping, through agitation at 25° C. for 2 hours, thereacted solution is analyzed in gas chromatography to find generation of0.839 mol of chrolotriethoxysilane. Expression 2 is employed to find ayield of 89.0% based on prepared Si.Si-based yield (mol %)=Produced chrolotriethoxysilane (mol)/(Preparedtetraethoxysilane (mol)+Prepared tetrachlorosilane (mol))  [Expression2]

In a 3 L four-neck flask equipped with an agitator, a nitrogenintroduction tube, a thermometer and a dropping funnel, 570 g (7.79 mol)of diethylamine is prepared and water-cooled, agitating and dropping thereacted mixture in nitrogen ambient for 30 minutes. The internaltemperature is kept at 25-30° C. during this process. After completionof dropping, through agitation for 2 hours, 1 L of n-heptane is added,followed by further agitation for 10 minutes. The reacted solution isfiltered under pressure, then condensed under reduced pressure, anddistilled under reduced pressure of 4 Torr at 62-63° C. in an Oldershowdistillation column with 10 logical stages. As a result, 144.3 g (0.613mol) of diethylaminotriethoxysilane is obtained. Expression 3 isemployed to find a yield of 65.0% based on prepared Si.Si-based yield (mol %)=Obtained diethylaminotriethoxysilane(mol)/(Prepared tetraethoxysilane (mol)+Prepared tetrachlorosilane(mol))  [Expression 3]

COMPARATIVE EXAMPLE 4

The reaction and operation are similarly performed as in Example 9except that 2.4 g of ethanol (5.5 mol % based on a total amount of Si)(0.052 mol) is employed. As a result, a yield of chlorotriethoxysilanein the reaction at the first step is 14.4% based on prepared Si, and anobtained yield of diethylaminotriethoxysilane through distillation afterthe reaction at the second step is 8.6% based on prepared Si.

COMPARATIVE EXAMPLE 5

The reaction and operation are similarly performed as in ComparativeExample 4 except that the reaction time is changed to 24 hrs. As aresult, a yield of chlorotriethoxysilane in the reaction at the firststep is 72.3% based on prepared Si, and an obtained yield ofdiethylaminotriethoxysilane through distillation after the reaction atthe second step is 52.2% based on prepared Si.

EXAMPLE 10

The reaction and operation are similarly performed as in Example 9except that 7.0 g of ethanol (16 mol % based on a total amount of Si)(0.15 mol) is employed. As a result, a yield of chlorotriethoxysilane inthe reaction at the first step is 87.5% based on prepared Si, and anobtained yield of diethylaminotriethoxysilane through distillation afterthe reaction at the second step is 63.9% based on prepared Si.

EXAMPLE 11

The reaction and operation are similarly performed as in Example 9except that 4.6 g of ethanol (11 mol % based on a total amount of Si)(0.10 mol) is employed and the reaction temperature at the first step ischanged to 40° C. As a result, a yield of chlorotriethoxysilane in thereaction at the first step is 78.2% based on prepared Si, and anobtained yield of diethylaminotriethoxysilane through distillation afterthe reaction at the second step is 57.3% based on prepared Si.

EXAMPLE 12

Commercially available 0.145 mol of SiCl₄ is supplied in a 100 mlfour-neck flask with previously nitrogen-replaced internal ambient, andcooled down to about 2° C. in ice bath. It is then agitated well while amicro feeder is employed for one hour to inject 0.440 mol of EtOH intoSiCl₄. In this case, a molar ratio of EtOH/SiCl₄ is 3.0. Duringinjection, the reaction temperature gradually lowers and finally reachesto −20° C. Then, through agitation for 3 hours, the reacted mixture isanalyzed in gas chromatography to find generation of 87% ClSi(OEt)₃based on prepared Si. Additionally, 125 ml of diethylamine is suppliedinto a 1000 ml flask with previously nitrogen-replaced internal ambientand, into the solution, the reacted mixture is dropped and agitated for3 hours at room temperature. Thereafter, the reacted mixture is analyzedin gas chromatography to find generation of Et₂NSi (OEt)₃ in an amountof 79% based on prepared Si.

From the results of Example 12 and Referential Example of Example 1, itis obvious like Example 1 that the yield at the first step in thecontinuous reactions is substantially a large factor that varies theyield as a whole. Therefore, in the following Referential Examples, thefirst step in the continuous reactions, that is, production oftrialkoxyhalo silanes, is described.

EXAMPLE 13

With a molar ratio EtOH/SiCl₄ of 3.4, the reaction of SiCl₄ with EtOH isperformed under the same operation as in Example 12. Then, the reactedmixture is analyzed in gas chromatography to find generation ofClSi(OEt)₃ in an amount of 57%.

EXAMPLE 14

With a molar ratio EtOH/SiCl₄ of 3.3, the reaction of SiCl₄ with EtOH isperformed under the same operation as in Example 12. Then, the reactedmixture is analyzed in gas chromatography to find generation ofClSi(OEt)₃ in an amount of 67%.

EXAMPLE 15

With a molar ratio EtOH/SiCl₄ of 3.2, the reaction of SiCl₄ with EtOH isperformed under the same operation as in Example 12. Then, the reactedmixture is analyzed in gas chromatography to find generation ofClSi(OEt)₃ in an amount of 77%.

EXAMPLE 16

With a molar ratio EtOH/SiCl₄ of 3.1, the reaction of SiCl₄ with EtOH isperformed under the same operation as in Example 12. Then, the reactedmixture is analyzed in gas chromatography to find generation ofClSi(OEt)₃ in an amount of 86%.

EXAMPLE 17

With a molar ratio EtOH/SiCl₄ of 3.05, the reaction of SiCl₄ with EtOHis performed under the same operation as in Example 12. Then, thereacted mixture is analyzed in gas chromatography to find generation ofClSi(OEt)₃ in an amount of 87%.

EXAMPLE 18

With a molar ratio EtOH/SiCl_(4 of) 2.95, the reaction of SiCl₄ withEtOH is performed under the same operation as in Example 12. Then, thereacted mixture is analyzed in gas chromatography to find generation ofClSi(OEt)₃ in an amount of 87%.

EXAMPLE 19

With a molar ratio EtOH/SiCl₄ of 2.9, the reaction of SiCl₄ with EtOH isperformed under the same operation as in Example 12. Then, the reactedmixture is analyzed in gas chromatography to find generation ofClSi(OEt)₃ in an amount of 90%.

EXAMPLE 20

With a molar ratio EtOH/SiCl₄ of 2.0, the reaction of SiCl₄ with EtOH isperformed under the same operation as in Example 12. Then, the reactedmixture is analyzed in gas chromatography to find generation ofClSi(OEt)₃ in an amount of 88%.

EXAMPLE 21

Examples of the polymerization or copolymerization catalysts ofα-olefins according to the present invention will be described belowthough the present invention is not limited at all by the description ofthe following Examples. In Examples 21-26, the polymerization activityrepresents a yield (g) of α-olefin polymers obtained in one hour ofpolymerization per 1 g of the solid catalyst. H. I. indicates aproportion (Weight of insoluble polymers/Weight of preparedpolymers×100) when α-olefin polymers are subjected to an extraction testin boiled n-heptane for 6 hours. A melt flow rate (MFR) is measuredbased on ASTM-D1238. It indicates the weight (g) of a melt polymer at230° C. under load of 2.16 Kg for 10 minutes. The melt flow rate isemployed as an index of hydrogen response. Namely, under condition ofα-olefin polymerization at the same hydrogen concentration, the higherthe numeral value the higher the hydrogen response becomes, and thelower the numeral value the lower the hydrogen response becomes. Themeso pentad fraction (mmmm) % obtained through examination ofmicro-tacticity or the index of stereomainity of α-olefin polymers iscalculated from a peak strength ratio in ¹³C-NMR spectrum belonging inpropylene polymers based on Macromolecules 8,687 (1975). The ¹³C-NMRspectrum is measured using a device EX-400 available from NipponElectronics with reference to TMS at a temperature of 130° C. in ano-dichlorobenzen solvent, scanning 8000 times.

The component [C] of the organosilicon compound is synthesized as shownbelow. First, into a four-neck flask having a 1 L volume and equippedwith a sufficiently nitrogen-replaced magnet seal agitator and adropping funnel, 0.14 mol of tetrachlorosilane, 0.34 mol oftetraethoxysilane and 0.022 mol of trifluoro acetate are introduced inturn. Then, they are subjected to reaction at room temperature for 3hours, and further subjected to reaction at 60° C. for 7 hours.Subsequently, 1.92 mol of diethylamine previously introduced into thedropping funnel is dropped. After completion of dropping, they aresubjected to reaction at room temperature for 9 hours. After completionof the reaction, the reacted solution is collected partly to confirmgeneration of the target product in gas chromatography. Thereafter, innitrogen ambient, the reacted solution in the flask is entirelytransferred into a container equipped with a G3 glass filter andsubjected to pressurized filtration with low-pressure nitrogen of 0.01MPa. Further, a hydrochloride of diethylamine of filtrated residue iscleaned and filtrated repeatedly with n-heptane until the target productcan not be confirmed in the filtrated solution. The cleaned mixture ofthe filtrated solution and the filtrated residue is condensed underreduced pressure to remove the solvent components such as n-heptanethrough distillation and collect the target product. The target producthas an appearance of colorless transparent liquid and a boiling point of58.0° C./mHg.

The purity of the component [C] is represented by wt. % derived from apeak area ratio in gas chromatography using a calibration curve. A gaschromatography device of GC-14A (available from Shimazu) is employed anda hydrogen flame ion detector is employed. A column of G-100, 20 m, 1.2mm inner diameter, 2 μm film thickness (available from GL Science) isemployed. An injection temperature and a detector temperature are at280° C. Under a temperature elevating condition, an initial columntemperature is kept at 70° C. for 10 minutes, then the temperature iselevated up to 260° C. at a rate of 16° C./min, and finally kept at 260°C. for 10 minutes.

As a result of the gas chromatography analysis under the abovecondition, the product has a composition of diethylamino triethoxysilane91.5 wt. %, diethylamine 0.1 wt. %, tetraethoxy silane 1.6 wt. %,diethylaminodiethoxymethoxysilane 1.1 wt. %,bis(diethylamino)diethoxysilane 5.2 wt. %, and hexaethoxy disiloxane 0.5wt. %. The products are identified in gas chromatography and massspectra thereof are shown in FIGS. 2-7.

As the solid catalyst component [A] for use in polymerization ofpropylene, a THC-TC type commercially available from Toho Catalyst isemployed. The Ti content is 1.7 wt. %.

Propylene is polymerized using an agitator-equipped autoclave ofstainless steel with a 2L inner volume. First, the interior of theautoclave is sufficiently replaced with nitrogen. Then, 0.0025 mmol ontitanium atom basis of n-heptane slurry of the solid catalyst component[A], 2 mmol of triethyl aluminum as the organoaluminum compoundcomponent [B], and 0.36 mmol of previously obtained purity 91.5 wt. %diethyl aminotriethoxysilane as the organosilicon compound component [C]are supplied in the autoclave. Subsequently, 0.4 MPa hydrogen and 1.2 Lliquidized propylene are introduced in turn. The interior of theautoclave is cooled down to 10° C., followed by preliminarypolymerization for 10 minutes. Subsequently, the temperature inside theautoclave is elevated up to 70° C., followed by further polymerizationat 70° C. for one hour under polymerization pressure of 3.8 MPa. Aftercompletion of the polymerization, non-reacted propylene gas isdischarged and the polymer is dried at 60° C. for 20 hours to producewhite powdery polypropylene. The results are shown in Table 1.

EXAMPLE 22

The organosilicon compound component [C] is synthesized as shown below.First, into a sufficiently nitrogen-replaced 1001 ml volume three-neckflask equipped with a dropping funnel, 30 ml of diethylamine isintroduced, and 0.015 mol of dichloro diethoxysilane previouslyintroduced into the dropping funnel is dropped therein at roomtemperature. After completion of dropping, 30 ml of diethylamine isadded and they are subjected to reaction at room temperature for 4hours. After completion of the reaction, the reacted solution iscollected partly to confirm generation of the target product in gaschromatography. Thereafter, in nitrogen ambient, the reacted solution inthe flask is entirely transferred into a container equipped with a G3glass filter and subjected to pressurized filtration with low-pressurenitrogen of 0.01 MPa. Further, a hydrochloride of diethylamine offiltrated residue is cleaned and filtrated repeatedly with diethylamineuntil the target product can not be confirmed in the filtrated solution.The cleaned mixture of the filtrated solution and the filtrated residueis condensed under reduced pressure to remove the solvent components andcollect the target product through distillation and purification. Thetarget product has an appearance of colorless transparent liquid and aboiling point of 109° C./9 mmHg. As a result of the gas chromatographyanalysis, the product has a composition ofbis(diethylamino)diethoxysilane 97.7 wt. %, diethylamine 0.7 wt. %,diethylaminodiethoxymethoxysilane 0.2 wt. %, diethylaminotriethoxysilane0.8 wt. %, and hexaethoxy disiloxane 0.6 wt. %.

The above resultant bis(diethylamino)diethoxysilane 97.7 wt. % is mixedwith the diethylaminotriethoxysilane 91.5 wt. % resulted from Example 1at a weight ratio of 1:1. Polymerization of propylene is performed as inExample 1 except that this mixture is employed as the component [C]. Theresults are shown in Table 1.

COMPARATIVE EXAMPLE 6

Polymerization of propylene is performed as in Example 1 except thatcyclohexylmethyldimethoxysilane is employed as the organosiliconcompound component [C]. The results are shown in Table 1. TABLE 1POLYMER- IZATION ACTIVITY MFR H.I mmmm g-PP/g-Cat. hr g/10 min % %EXAMPLE 21 41,400 400 96.8 98.8 EXAMPLE 22 41,500 533 95.6 98.6COMPARATIVE 42,600 76.5 97 98.2 EXAMPLE 6

EXAMPLE 23

Polymerization of propylene is implemented as follows. First, a 2L innervolume stainless steel autoclave equipped with a magnet seal agitator issufficiently nitrogen-replaced in the interior thereof. Into theautoclave, 2.2 mmol of triethyl aluminum as the organoaluminum compoundcomponent [B], 0.36 mmol of dietylaminotirethoxysilane resulted from thepresent invention as the component [C], and 2.5×10⁻³ mmol of n-heptaneslurry on titanium atom basis as the solid catalyst component [A]of theTHC-JC type available from Toho Catalyst are introduced in turn. Then,hydrogen (0.4 MPa) and liquidized propylene(1.2 L) are introduced.Subsequently, the temperature inside the autoclave is elevated up to 70°C., followed by polymerization at 70° C. for one hour underpolymerization pressure of 3.8 MPa. After completion of thepolymerization, non-reacted propylene gas is discharged and the polymeris dried at 60° C. for 20 hours to produce white powdery polypropylene.The polymerization activity is 42 kg/g-Cat. hr, MFR is 400 g/10 min, H.Iis 96.2%, and mmmm is 98.8%.

EXAMPLE 24

The solid catalyst component [A] for use in polymerization of propyleneis the THC-JC type available from Toho Catalyst. The content of Ti is1.7 wt. %.

Propylene is polymerized using an agitator-equipped autoclave ofstainless steel with a 2L inner volume. First, the interior of theautoclave is sufficiently replaced with nitrogen. Then, 0.0025 mmol ontitanium atom basis of n-heptane slurry of the solid catalyst component[A], 0.36 mmol of chlortriethoxysilane and 0.72 mmol of diethylamine asthe (C) component, and 2 mmol of triethyl aluminum as the (B) componentare supplied in the autoclave. Subsequently, 0.4 MPa hydrogen and 1.2 Lliquidized propylene are introduced in turn. The interior of theautoclave is cooled down to 10° C., followed by preliminarypolymerization for 10 minutes. Subsequently, the temperature inside theautoclave is elevated up to 70° C., followed by further polymerizationat 70° C. for one hour under polymerization pressure of 3.8 MPa. Aftercompletion of the polymerization, non-reacted propylene gas isdischarged and the polymer is dried at 60° C. for 20 hours to producewhite powdery polypropylene. The polymerization activity is 35,800g-PP/g-Ct. hr. MFR is 615, H.I is 95.9, and the meso pentad fraction(mmmm) is 97.9.

EXAMPLE 25

As the component (C), the reacted mixture additionally mixed withchlortriethoxysilane and diethylamine and filtrated is employed whileothers are similar to those in Example 1. The polymerization activity is41,800 g-PP/g-Ct. hr, MFR is 400, H.I is 96.6, and the meso pentadfraction (mmmm) is 98.5.

EXAMPLE 26

As the component (C), the reacted mixture additionally mixed with 0.36mmol of chlortriethoxysilane and 0.72 mmol of diethylamine and filtratedis employed while others are similar to those in Example 2. Thepolymerization activity is 43,400 g-PP/g-Ct. hr, MFR is 444, H.I is96.2, and the meso pentad fraction (mmmm) is 98.4.

EXAMPLE 27

As the component (B), only chlortriethoxysilane is employed anddiethylamine is not employed while others are similar to those inExample 1. The polymerization activity is 32,900 g-PP/g-Ct. hr, MFR is799, H.I is 94.9, and the meso pentad fraction (mmmm) is 97.5.

1-22. (canceled)
 23. A process for production of trialkoxyhalosilanes,which comprises reacting a tetrahalosilane represented by Formula 1 witha tetraalkoxysilane represented by Formula 2 in the mixture of analcohol composed of the same alkoxy group as that of thetetraalkoxysilane to yield a trialkoxyhalosilane represented by Formula3, wherein the alcohol is used in an amount of 5-50% by mol based on atotal amount of Si in the tetrahalosilane and the tetraalkoxysilane:SiX₄  [Formula 1] (where X denotes halogen)Si(OR¹)₄  [Formula 2] (where R¹ denotes a hydrocarbon group having 1-6carbon atoms)XSi(OR¹)₃  [Formula 3] (where X denotes halogen; and R¹ a hydrocarbongroup having 1-6 carbon atoms).
 24. The process for production oftrialkoxyhalosilanes according to claim 23, wherein a molar quantity ofthe tetraalkoxysilane in use is more than three times the molar quantityof the tetrahalosilane in use.
 25. The process for production oftrialkoxyhalosilanes according to claim 23, wherein X is chlor and R¹ isethyl in the compound represented by Formulae 1-3.
 26. The process forproduction of trialkoxyhalosilanes according to claim 24, wherein X ischlor and R¹ is ethyl in the compound represented by Formulae 1-3.
 27. Aprocess for production of trialkoxyhalosilanes, which comprises reactinga tetrahalosilane represented by Formula 4 with an alcohol representedby Formula 5 at a controlled temperature of 40° C. or below to yield atrialkoxyhalosilane represented by Formula 6:SiX₄  [Formula 4] (where X denotes halogen)R¹OH  [Formula 5] (where R¹ denotes a hydrocarbon group having 1-6carbon atoms)XSi(OR¹)₃  [Formula 6] (where X denotes halogen; and R¹ a hydrocarbongroup having 1-6 carbon atoms).
 28. The process for production oftrialkoxyhalosilanes according to claim 27, wherein the reaction of thetetrahalosilane with the alcohol is performed in the presence of an acidcatalyst.
 29. The process for production of trialkoxyhalosilanesaccording to claim 28, wherein the acid catalyst is a hydrogen halidesecondarily produced in the reaction.
 30. The process for production oftrialkoxyhalosilanes according to claim 27, wherein X is chlor and R¹ isethyl in the compound represented by Formulae 4-6.
 31. The process forproduction of trialkoxyhalosilanes according to claim 28, wherein X ischlor and R¹ is ethyl in the compound represented by Formulae 4-6. 32.The process for production of trialkoxyhalosilanes according to claim29, wherein X is chlor and R¹ is ethyl in the compound represented byFormulae 4-6.
 33. A process for production of trialkoxy(dialkylamino)silanes, which comprises a first step including the process forproduction of trialkoxyhalosilanes according to claim 23; and a secondstep of reacting the trialkoxy halosilane obtained in the first stepwith a dialkylamine represented by Formula 7 to yield atrialkoxy(dialkylamino) silane represented by Formula 8:R²R³NH  [Formula 7] (where R² denotes a hydrocarbon group having 1-12carbon atoms; and R³ a hydrocarbon group having 1-12 carbon atoms)R²R³NSi(OR¹)₃  [Formula 8] (where R¹ denotes a hydrocarbon group having1-6 carbon atoms; R² a hydrocarbon group having 1-12 carbon atoms; andR³ a hydrocarbon group having 1-12 carbon atoms).
 34. The process forproduction of trialkoxy(dialkylamino) silanes according to claim 33,wherein the reacted mixture obtained in the first step is reacted withthe dialkylamine represented by Formula 7, without subjecting toisolation/purification.
 35. The process for production oftrialkoxy(dialkylamino) silanes according to claim 33, wherein X ischlor and R¹, R² and R³ are ethyl in the compound represented byFormulae 1-8.
 36. The process for production of trialkoxy(dialkylamino)silanes according to claim 34, wherein X is chlor and R¹, R² and R³ areethyl in the compound represented by Formulae 1-8.
 37. A catalystcomponent for polymerization or copolymerization catalysts of α-olefins,which comprises a mixture of silane compounds represented by Formulae 9and 10:Si(OR¹)₃R²  [Formula 9] (where R¹ denotes a hydrocarbon group having 2-6carbon atoms; and R² a hydrocarbon group having 1-12 carbon atoms, anamino group including a hydrogen atom and a hydrocarbon group having1-12 carbon atoms, which are bonded on a N atom, or an amino groupincluding two hydrocarbon groups each having 1-12 carbon atoms, whichare bonded on a N atom (the two hydrocarbon groups may be the same ordifferent from each other))SiR³ ₄  [Formula 10] (where R³ denotes an alkoxy group having 1-6 carbonatoms, a hydrocarbon group having 1-12 carbon atoms, an amino groupincluding a hydrogen atom and a hydrocarbon group having 1-12 carbonatoms, which are bonded on a N atom, or an amino group including twohydrocarbon groups each having 1-12 carbon atoms, which are bonded on aN atom (the two hydrocarbon groups may be the same or different fromeach other). Each R³ may be the same as or different from another.Formulae 9 and 10 do not represent the same compound).
 38. A catalystcomponent for polymerization or copolymerization catalysts of α-olefins,which comprises a mixture of silane compounds represented by Formulae 11and 12:Si(OR¹)₃(NR⁴R⁵)  [Formula 11] (where R¹ denotes a hydrocarbon grouphaving 2-6 carbon atoms; R⁴ a hydrocarbon group having 1-12 carbonatoms, or a hydrogen atom; and R⁵ a hydrocarbon group having 1-12 carbonatoms)Si(R⁶)_(n)(NR⁷R⁸)_(4-n)  [Formula 12] (where R⁶ denotes a hydrocarbongroup having 1-12 carbon atoms or an alkoxy group having 1-6 carbonatoms (each R⁶ may be the same as or different from another); R⁷ ahydrocarbon group having 1-12 carbon atoms; R⁸ a hydrocarbon grouphaving 1-12 carbon atoms; and n is equal to 1-2 or 4).
 39. The catalystcomponent for polymerization or copolymerization catalysts of α-olefinsaccording to claim 37, wherein the silane compound represented byFormulae 9-12 is obtained by reacting a tetrahalosilane represented byFormula 13 with a tetraalkoxysilane represented by Formula 14 to yield atrialkoxyhalosilane represented by Formula 15, which is then reactedwith a dialkylamine represented by Formula 16:SiX₄  [Formula 13] (where X denotes halogen)Si(OR¹)₄  [Formula 14] (where R¹ denotes a hydrocarbon group having 2-6carbon atoms)XSi(OR¹)₃  [Formula 15] (where X denotes halogen; and R¹ a hydrocarbongroup having 2-6 carbon atoms)R²R³NH  [Formula 16] (where R² denotes a hydrocarbon group having 1-12carbon atoms; and R³ a hydrocarbon group having 1-12 carbon atoms). 40.The catalyst component for polymerization or copolymerization catalystsof α-olefins according to claim 38, wherein the silane compoundrepresented by Formulae 9-12 is obtained by reacting a tetrahalosilanerepresented by Formula 13 with a tetraalkoxysilane represented byFormula 14 to yield a trialkoxyhalosilane represented by Formula 15,which is then reacted with a dialkylamine represented by Formula 16:SiX₄  [Formula 13] (where X denotes halogen)Si(OR¹)₄  [Formula 14] (where R¹ denotes a hydrocarbon group having 2-6carbon atoms)XSi(OR¹)₃  [Formula 15] (where X denotes halogen; and R¹ a hydrocarbongroup having 2-6 carbon atoms)R²R³NH  [Formula 16] (where R² denotes a hydrocarbon group having 1-12carbon atoms; and R³ a hydrocarbon group having 1-12 carbon atoms). 41.A catalyst component for polymerization or copolymerization catalysts ofα-olefins, which comprises a mixture of a diethylaminotriethoxysilaneand a bis(diethylamino)diethoxysilane.
 42. A polymerization orcopolymerization catalyst of α-olefins, which includes the catalystcomponent according to claim
 37. 43. A polymerization orcopolymerization catalyst of α-olefins, which includes the catalystcomponent according to claim
 38. 44. A polymerization orcopolymerization catalyst of α-olefins, which includes the catalystcomponent according to claim
 39. 45. A polymerization orcopolymerization catalyst of α-olefins, which includes the catalystcomponent according to claim
 40. 46. A polymerization orcopolymerization catalyst of α-olefins, which includes the catalystcomponent according to claim
 41. 47. A polymerization orcopolymerization catalyst of α-olefins, which comprises [A] a solidcatalyst component essentially including magnesium, titanium, a halogenelement and an electron donor; [B] an organoaluminum compound component;and [C] the catalyst component according to claim
 37. 48. Apolymerization or copolymerization catalyst of α-olefins, whichcomprises [A] a solid catalyst component essentially includingmagnesium, titanium, a halogen element and an electron donor; [B] anorganoaluminum compound component; and [C] the catalyst componentaccording to claim
 38. 49. A polymerization or copolymerization catalystof α-olefins, which comprises [A] a solid catalyst component essentiallyincluding magnesium, titanium, a halogen element and an electron donor;[B] an organoaluminum compound component; and [C] the catalyst componentaccording to claim
 39. 50. A polymerization or copolymerization catalystof α-olefins, which comprises [A] a solid catalyst component essentiallyincluding magnesium, titanium, a halogen element and an electron donor;[B] an organoaluminum compound component; and [C] the catalyst componentaccording to claim
 40. 51. A polymerization or copolymerization catalystof α-olefins, which comprises [A] a solid catalyst component essentiallyincluding magnesium, titanium, a halogen element and an electron donor;[B] an organoaluminum compound component; and [C] the catalyst componentaccording to claim
 41. 52. A process for polymerization of α-olefins,which comprises polymerizing or copolymerizing an α-olefin in thepresence of the catalyst according to claim
 42. 53. A process forpolymerization of α-olefins, which comprises polymerizing orcopolymerizing an α-olefin in the presence of the catalyst according toclaim
 43. 54. A process for polymerization of α-olefins, which comprisespolymerizing or copolymerizing an α-olefin in the presence of thecatalyst according to claim
 44. 55. A process for polymerization ofα-olefins, which comprises polymerizing or copolymerizing an α-olefin inthe presence of the catalyst according to claim
 45. 56. A process forpolymerization of α-olefins, which comprises polymerizing orcopolymerizing an α-olefin in the presence of the catalyst according toclaim
 46. 57. A process for polymerization of α-olefins, which comprisespolymerizing or copolymerizing an α-olefin in the presence of thecatalyst according to claim
 47. 58. A process for polymerization ofα-olefins, which comprises polymerizing or copolymerizing an α-olefin inthe presence of the catalyst according to claim
 48. 59. A process forpolymerization of α-olefins, which comprises polymerizing orcopolymerizing an α-olefin in the presence of the catalyst according toclaim
 49. 60. A process for polymerization of α-olefins, which comprisespolymerizing or copolymerizing an α-olefin in the presence of thecatalyst according to claim
 50. 61. A process for polymerization ofα-olefins, which comprises polymerizing or copolymerizing an α-olefin inthe presence of the catalyst according to claim
 51. 62. A catalystcomponent for polymerization or copolymerization catalysts of α-olefins,which comprises a reacted mixture of a trialkoxyhalosilane representedby Formula 17 with a dialkylamine represented by Formula 18:XSi(OR¹)₃  [Formula 17] (where X denotes halogen; and R¹ denotes ahydrocarbon group having 2-6 carbon atoms)R²R³NH  [Formula 18] (where R² denotes a hydrocarbon group having 1-12carbon atoms; and R³ a hydrocarbon group having 1-12 carbon atoms). 63.A polymerization or copolymerization catalyst of α-olefins, whichincludes the catalyst component according to claim
 62. 64. Apolymerization or copolymerization catalyst of α-olefins, whichcomprises [A] a solid catalyst component essentially includingmagnesium, titanium, a halogen element and an electron donor; [B] anorganoaluminum compound component; and [C] the catalyst componentaccording to claim
 62. 65. The polymerization or copolymerizationcatalyst of α-olefins according to claim 63, wherein the reacted mixtureof the trialkoxyhalosilane represented by Formula 17 with thedialkylamine represented by Formula 18 is employed without subjecting toisolation/purification.
 66. The polymerization or copolymerizationcatalyst of α-olefins according to claim 64, wherein the reacted mixtureof the trialkoxyhalosilane represented by Formula 17 with thedialkylamine represented by Formula 18 is employed without subjecting toisolation/purification.
 67. A process for polymerization of α-olefins,which comprises polymerizing or copolymerizing an α-olefin in thepresence of the catalyst according to claim
 63. 68. A process forpolymerization of α-olefins, which comprises polymerizing orcopolymerizing an α-olefin in the presence of the catalyst according toclaim
 64. 69. A process for polymerization of α-olefins, which comprisespolymerizing or copolymerizing an α-olefin in the presence of thecatalyst according to claim 65.